Deep-ultraviolet (DUV) nonlinear-optical (NLO) materials generating coherent DUV light by a direct second-harmonic-generation (SHG) process have long been pursued as industrially useful lasers. For several decades, KBe2BO3F2 (KBBF) has been regarded as the best DUV-NLO material; it is characterized by a short DUV phase-matching edge of 161 nm and a large SHG coefficient of 0.47 pm/V. However, it suffers a strong layering tendency, hindering the growth of large crystals for commercial use. Here, we use a computer-aided swarm structure searching technique to design an alternative DUV-NLO material with a new atmospheric-pressure phase Be2BO3F2 with a P (6) over bar 2c space group (gamma-BBF) that outperforms the DUV-NLO properties of KBBF. The predicted DUV phase-matching edge and SHG coefficient of gamma-BBF are 152 rim and 0.70 pm/V, respectively. The structure of gamma-BBF reduces the layering tendency compared with KBBF because of the absence of K atoms in the gamma-BBF crystal. Our work paves the way for superior DUV-NLO materials that can be grown as large crystals for commercial applications.